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<p>Dynamic chemistry offers opportunities for the design of smart materials that can self adapt or self repair to mediate their functionality. However, achieving anti-crack toughness using dynamic covalent bonds is often overlooked in crystalline porous solids such as metal–organic frameworks. Here we propose that crystalline dynamicity can be derived from bio-inspired disulfide metathesis, as demonstrated by a dynamic combinatorial library of isomeric metal–organic frameworks (LIFM-105, LIFM-105i, and LIFM-105a). Sulfur–sulfur bond breakage and regeneration facilitate stimuli-responsive interconversion between two-dimensional and three-dimensional frameworks, involving simultaneous layer rotation, component shift and linkage reorganization. The disulfide exchange-based crystal dynamics provides these porous solids with gas-induced adaptiveness and the gate effect, enabling pore tuning for efficient removal of C<sub>2</sub>H<sub>2</sub> from C<sub>2</sub>H<sub>4</sub>. Additionally, the guest-adaptation-motivated restoration and reorganization of the ‘damaged’ frameworks afford a promising protocol to apply radical-mediated dynamic solids as adaptive porous materials for durable separation and other applications.</p><p></p>

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Adaptive metal–organic frameworks with crystalline dynamicity for durable gas separation

  • 期刊论文

  • 发表日期：

    2025年10月24日

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  • Cheng-Xia Chen,
  • Xili Cui,
  • Yang-Yang Xiong,
  • Pui Ching Lan,
  • Kui Tan,
  • Zhang-Wen Wei,
  • Zheng Niu,
  • Chuan Shan,
  • Lifeng Yang,
  • Shengqian Ma,
  • Cheng-Yong Su

摘要

Dynamic chemistry offers opportunities for the design of smart materials that can self adapt or self repair to mediate their functionality. However, achieving anti-crack toughness using dynamic covalent bonds is often overlooked in crystalline porous solids such as metal–organic frameworks. Here we propose that crystalline dynamicity can be derived from bio-inspired disulfide metathesis, as demonstrated by a dynamic combinatorial library of isomeric metal–organic frameworks (LIFM-105, LIFM-105i, and LIFM-105a). Sulfur–sulfur bond breakage and regeneration facilitate stimuli-responsive interconversion between two-dimensional and three-dimensional frameworks, involving simultaneous layer rotation, component shift and linkage reorganization. The disulfide exchange-based crystal dynamics provides these porous solids with gas-induced adaptiveness and the gate effect, enabling pore tuning for efficient removal of C2H2 from C2H4. Additionally, the guest-adaptation-motivated restoration and reorganization of the ‘damaged’ frameworks afford a promising protocol to apply radical-mediated dynamic solids as adaptive porous materials for durable separation and other applications.